Journal
NATURE CHEMISTRY
Volume 10, Issue 2, Pages 177-183Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2910
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Funding
- Photosynthetic Antenna Research Center, an Energy Frontier Research Center - Basic Energy Sciences programme of the US Department of Energy Office of Science [DE-SC0001035]
- European Community (H2020 Marie Sklodowska-Curie Actions) [655059]
- CIFAR
- Canadian Institute for Advanced Research through Bio-Inspired Solar Energy programme
- Marie Curie Actions (MSCA) [655059] Funding Source: Marie Curie Actions (MSCA)
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Femtosecond pulsed excitation of light-harvesting complexes creates oscillatory features in their response. This phenomenon has inspired a large body of work aimed at uncovering the origin of the coherent beatings and possible implications for function. Here we exploit site-directed mutagenesis to change the excitonic level structure in Fenna-Matthews-Olson (FMO) complexes and compare the coherences using broadband pump-probe spectroscopy. Our experiments detect two oscillation frequencies with dephasing on a picosecond timescale-both at 77 K and at room temperature. By studying these coherences with selective excitation pump-probe experiments, where pump excitation is in resonance only with the lowest excitonic state, we show that the key contributions to these oscillations stem from groundstate vibrational wavepackets. These experiments explicitly show that the coherences-although in the ground electronic state-can be probed at the absorption resonances of other bacteriochlorophyll molecules because of delocalization of the electronic excitation over several chromophores.
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